Pressure tuning of Kitaev spin liquid candidate Na3Co2SbO6

E. H.T. Poldi; R. Tartaglia; G. Fabbris; N. Nguyen; H. Park; Z. Liu; M. van Veenendaal; R. Kumar; G. Jose; S. Samanta; W. Bi; Y. Xiao; D. Popov; Y. Wu; J. W. Kim; H. Zheng; J. Yan; J. F. Mitchell; R. J. Hemley; D. Haskel

doi:10.1038/s42005-025-02174-2

Pressure tuning of Kitaev spin liquid candidate Na₃Co₂SbO₆

E. H.T. Poldi, R. Tartaglia, G. Fabbris, N. Nguyen, H. Park, Z. Liu, M. van Veenendaal, R. Kumar, G. Jose, S. Samanta, W. Bi, Y. Xiao, D. Popov, Y. Wu, J. W. Kim, H. Zheng, J. Yan, J. F. Mitchell, R. J. Hemley, D. Haskel

Research output: Contribution to journal › Article › peer-review

Abstract

The search for Kitaev’s quantum spin liquid in real materials has recently expanded with the prediction that honeycomb lattices of divalent, high-spin cobalt ions could host the dominant bond-dependent exchange interactions required to stabilize the elusive entangled quantum state. The layered honeycomb Na₃Co₂SbO₆ has been singled out as a leading candidate provided that the trigonal crystal field acting on Co 3d orbitals, which enhances non-Kitaev exchange interactions between Jeff=12 spin-orbital pseudospins, is reduced. Here we show that applied pressure leads to anisotropic compression of the layered structure, significantly reducing the trigonal distortion of CoO₆ octahedra. Ferromagnetic correlations between pseudospins are enhanced in the spin-polarized (3 Tesla) phase up to about 60 GPa. Higher pressures drive a high-spin to low-spin transition destroying the Jeff=12 moments required to map the spin Hamiltonian into Kitaev’s model. The spin transition strongly suppresses the low-temperature magnetic susceptibility and appears to stabilize a paramagnetic phase driven by frustration. The possible emergence of frustrated magnetism of localized S=12 moments opens the door for exploration of novel magnetic quantum states in compressed honeycomb lattices of divalent cobaltates.

Original language	English
Article number	310
Journal	Communications Physics
Volume	8
Issue number	1
DOIs	https://doi.org/10.1038/s42005-025-02174-2
State	Published - Dec 2025

Funding

The authors thank Hide Takagi and Janice Musfeldt for helpful discussions. Work at the Advanced Photon Source (APS) and Materials Science Division of Argonne National Laboratory (ANL) was supported by the U.S. DOE Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Work at UIC was supported by the U.S. National Science Foundation (NSF, DMR-210488), the U.S. Department of Energy-National Nuclear Security Administration (DOE-NNSA) through the Chicago/DOE Alliance Center (DE-NA0004153), and the DOE Office of Science (DE-SC0020340). Portions of this work were performed at HPCAT (Sector 16) of APS at ANL. HPCAT operations are supported by DOE-NNSA’s Office of Experimental Sciences. Helium and neon pressure media were loaded at GeoSoilEnviroCARS (The University of Chicago, Sector 13), APS, ANL. GeoSoilEnviroCARS is supported by NSF-Earth Sciences (EAR-1634415) and DOE-GeoSciences (DE-FG02-94ER14466). Crystal growth at ORNL was supported by the U.S. DOE, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Neutron scattering research used resources at ORNL’s High Flux Isotope Reactor, a DOE Office of Science User Facility, with beamtime allocated to the WAND instrument. R.T. was supported by the São Paulo Research Foundation (FAPESP, 2019/10401-9 and 2022/03539-7). H.P. acknowledges the support by the Materials Sciences and Engineering Division, Basic Energy Sciences, Office of Science, US DOE. We acknowledge the computing resources provided on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at ANL. This research used the 22-IR-1 beamline (FIS) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704, and also supported by DOE-NNSA (CDAC) and the NSF grant EAR-2223273 (Synchrotron Earth and Environmental Science, SEES). Work at UAB was supported by NSF CAREER Award No. DMR-2045760. The authors thank Hide Takagi and Janice Musfeldt for helpful discussions. Work at the Advanced Photon Source (APS) and Materials Science Division of Argonne National Laboratory (ANL) was supported by the U.S. DOE Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. Work at UIC was supported by the U.S. National Science Foundation (NSF, DMR-210488), the U.S. Department of Energy-National Nuclear Security Administration (DOE-NNSA) through the Chicago/DOE Alliance Center (DE-NA0004153), and the DOE Office of Science (DE-SC0020340). Portions of this work were performed at HPCAT (Sector 16) of APS at ANL. HPCAT operations are supported by DOE-NNSA’s Office of Experimental Sciences. Helium and neon pressure media were loaded at GeoSoilEnviroCARS (The University of Chicago, Sector 13), APS, ANL. GeoSoilEnviroCARS is supported by NSF-Earth Sciences (EAR-1634415) and DOE-GeoSciences (DE-FG02-94ER14466). Crystal growth at ORNL was supported by the U.S. DOE, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Neutron scattering research used resources at ORNL’s High Flux Isotope Reactor, a DOE Office of Science User Facility, with beamtime allocated to the WAND2 instrument. R.T. was supported by the São Paulo Research Foundation (FAPESP, 2019/10401-9 and 2022/03539-7). H.P. acknowledges the support by the Materials Sciences and Engineering Division, Basic Energy Sciences, Office of Science, US DOE. We acknowledge the computing resources provided on Bebop, a high-performance computing cluster operated by the Laboratory Computing Resource Center at ANL. This research used the 22-IR-1 beamline (FIS) of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704, and also supported by DOE-NNSA (CDAC) and the NSF grant EAR-2223273 (Synchrotron Earth and Environmental Science, SEES). Work at UAB was supported by NSF CAREER Award No. DMR-2045760.

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Poldi, E. H. T., Tartaglia, R., Fabbris, G., Nguyen, N., Park, H., Liu, Z., van Veenendaal, M., Kumar, R., Jose, G., Samanta, S., Bi, W., Xiao, Y., Popov, D., Wu, Y., Kim, J. W., Zheng, H., Yan, J., Mitchell, J. F., Hemley, R. J., & Haskel, D. (2025). Pressure tuning of Kitaev spin liquid candidate Na₃Co₂SbO₆. Communications Physics, 8(1), Article 310. https://doi.org/10.1038/s42005-025-02174-2

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title = "Pressure tuning of Kitaev spin liquid candidate Na3Co2SbO6",

abstract = "The search for Kitaev{\textquoteright}s quantum spin liquid in real materials has recently expanded with the prediction that honeycomb lattices of divalent, high-spin cobalt ions could host the dominant bond-dependent exchange interactions required to stabilize the elusive entangled quantum state. The layered honeycomb Na3Co2SbO6 has been singled out as a leading candidate provided that the trigonal crystal field acting on Co 3d orbitals, which enhances non-Kitaev exchange interactions between Jeff=12 spin-orbital pseudospins, is reduced. Here we show that applied pressure leads to anisotropic compression of the layered structure, significantly reducing the trigonal distortion of CoO6 octahedra. Ferromagnetic correlations between pseudospins are enhanced in the spin-polarized (3 Tesla) phase up to about 60 GPa. Higher pressures drive a high-spin to low-spin transition destroying the Jeff=12 moments required to map the spin Hamiltonian into Kitaev{\textquoteright}s model. The spin transition strongly suppresses the low-temperature magnetic susceptibility and appears to stabilize a paramagnetic phase driven by frustration. The possible emergence of frustrated magnetism of localized S=12 moments opens the door for exploration of novel magnetic quantum states in compressed honeycomb lattices of divalent cobaltates.",

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AU - Poldi, E. H.T.

AU - Tartaglia, R.

AU - Fabbris, G.

AU - Nguyen, N.

AU - Park, H.

AU - Liu, Z.

AU - van Veenendaal, M.

AU - Kumar, R.

AU - Jose, G.

AU - Samanta, S.

AU - Bi, W.

AU - Xiao, Y.

AU - Popov, D.

AU - Wu, Y.

AU - Kim, J. W.

AU - Zheng, H.

AU - Yan, J.

AU - Mitchell, J. F.

AU - Hemley, R. J.

AU - Haskel, D.

N1 - Publisher Copyright: © UChicago Argonne, LLC, Operator of Argonne National Laboratory, under exclusive licence to Springer Nature Limited 2025.

PY - 2025/12

Y1 - 2025/12

N2 - The search for Kitaev’s quantum spin liquid in real materials has recently expanded with the prediction that honeycomb lattices of divalent, high-spin cobalt ions could host the dominant bond-dependent exchange interactions required to stabilize the elusive entangled quantum state. The layered honeycomb Na3Co2SbO6 has been singled out as a leading candidate provided that the trigonal crystal field acting on Co 3d orbitals, which enhances non-Kitaev exchange interactions between Jeff=12 spin-orbital pseudospins, is reduced. Here we show that applied pressure leads to anisotropic compression of the layered structure, significantly reducing the trigonal distortion of CoO6 octahedra. Ferromagnetic correlations between pseudospins are enhanced in the spin-polarized (3 Tesla) phase up to about 60 GPa. Higher pressures drive a high-spin to low-spin transition destroying the Jeff=12 moments required to map the spin Hamiltonian into Kitaev’s model. The spin transition strongly suppresses the low-temperature magnetic susceptibility and appears to stabilize a paramagnetic phase driven by frustration. The possible emergence of frustrated magnetism of localized S=12 moments opens the door for exploration of novel magnetic quantum states in compressed honeycomb lattices of divalent cobaltates.

AB - The search for Kitaev’s quantum spin liquid in real materials has recently expanded with the prediction that honeycomb lattices of divalent, high-spin cobalt ions could host the dominant bond-dependent exchange interactions required to stabilize the elusive entangled quantum state. The layered honeycomb Na3Co2SbO6 has been singled out as a leading candidate provided that the trigonal crystal field acting on Co 3d orbitals, which enhances non-Kitaev exchange interactions between Jeff=12 spin-orbital pseudospins, is reduced. Here we show that applied pressure leads to anisotropic compression of the layered structure, significantly reducing the trigonal distortion of CoO6 octahedra. Ferromagnetic correlations between pseudospins are enhanced in the spin-polarized (3 Tesla) phase up to about 60 GPa. Higher pressures drive a high-spin to low-spin transition destroying the Jeff=12 moments required to map the spin Hamiltonian into Kitaev’s model. The spin transition strongly suppresses the low-temperature magnetic susceptibility and appears to stabilize a paramagnetic phase driven by frustration. The possible emergence of frustrated magnetism of localized S=12 moments opens the door for exploration of novel magnetic quantum states in compressed honeycomb lattices of divalent cobaltates.

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Pressure tuning of Kitaev spin liquid candidate Na₃Co₂SbO₆

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